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Journal of Environmental Management 320 (2022) 115887

Contents lists available at ScienceDirect

Journal of Environmental Management


journal homepage: www.elsevier.com/locate/jenvman

Review

A critical review of the pre-processing and metals recovery methods from


e-wastes
Rima Kumari, Sukha Ranjan Samadder *
Department of Environmental Science & Engineering, Indian Institute of Technology (Indian School of Mines), Dhanbad, 826004, India

A R T I C L E I N F O A B S T R A C T

Keywords: E-wastes being potential sources of numerous valuable metals are promoted to undergo recycling and recovery
Biometallurgical method under the umbrella of urban mining and circular economy. Thus, the present study provides a critical review of
E-wastes the technological details of different metal recycling processes, pre-treatment methods, and the advancements
Hydrometallurgical method
made in these techniques. Critical evaluation of different metal recovery techniques has also been presented
Metal recovery
based on the available life cycle assessment (LCA), techno-economic, and industrial-scale studies. The study
And Pre-processing techniques
revealed that the integrated metal recovery techniques serve better in terms of recovery efficiency and envi­
ronmental performance than any single recovery technique. Also, scaling up of biometallurgical, electro­
chemical, and super critical fluid extraction methods needs to be promoted due to their better environmental
performances.

1. Introduction even higher in e-wastes than that in their natural ores. Thus, recovery of
these valuable metals from e-wastes is considered as feasible solution
The rapid advancements in technology, urbanization, affluence, from both economy and environment point of view.
economic growth, and transition to online mode upon COVID-19 Recycling and recovery of useable components from the wastes have
pandemic are some of the factors responsible for increase in demand always been considered as wise and sustainable step of managing them.
for different electrical and electronic products (EEPs). The rising de­ When this recovery is done formally, it provides myriad benefits
mand for these EEPs can be linked directly with their higher rate of extending from waste reduction to energy-saving and from emission
obsolescence. This can be validated by the fact that a record of 53.6 reduction to economic benefits (Yang et al., 2020). Despite several
million metric tons (Mt) of e-waste has been generated worldwide in benefits, the formal sector has managed to collect and recycle only
2019 which grew by 9.2 Mt since 2014 and is expected to surpass the 17.4% of the total e-wastes generated globally in 2019 indicating the
projected e-waste generation rate of 74.7 Mt by 2030 (Forti et al., 2020). channelization of these wastes either in landfills or into informal recy­
The enhanced rate of e-waste generation creates huge problem for its cling system (Forti et al., 2020). These routes often involve a set of
effective management. pre-activities that are intended to be applied as an effective waste
E-wastes are the whole or part of EEPs or rejects from their management option; however, they are not considered sustainable and
manufacturing and repairing processes that are no longer of use and are suitable from an environmental perspective. Apparently, it becomes
intended to be discarded (MoEF&CC, 2016). These wastes consist of a crucial to recover the different valuable elements from these wastes
diverse range of EEPs as shown in Table 1, which contain a broad while, undertaking both economical as well as environmental aspects at
spectrum of different organic and inorganic substances including metals, the same time.
plastics, ceramics, etc. (Fig. 1). The composition of e-wastes varies Different conventional techniques such as pyrometallurgy and hy­
depending on their type, age, and manufacturing company. Table 2 drometallurgy are the major recycling techniques that have been
shows the percentage distribution of different valuable metals in currently adopted in most of the countries; however, these techniques
different types of e-wastes along with their estimated economic values have serious concerns mainly in the form of toxicological effects and
revealing the recovery potential of these e-wastes. The concentration of secondary environmental pollution. The bottlenecks of these techniques
these metals (especially the precious metals such as Au, Ag, Pt, and Pd) is have resulted in the quest for the development of safer and more eco-

* Corresponding author.
E-mail addresses: rima07km@gmail.com (R. Kumari), samadder@iitism.ac.in (S.R. Samadder).

https://doi.org/10.1016/j.jenvman.2022.115887
Received 28 January 2022; Received in revised form 24 July 2022; Accepted 25 July 2022
Available online 5 August 2022
0301-4797/© 2022 Elsevier Ltd. All rights reserved.
R. Kumari and S.R. Samadder Journal of Environmental Management 320 (2022) 115887

Table 1 friendly techniques. Moreover, the realization of the importance of the


Different categories of e-wastes. recovery potential of numerous invaluable resources from these e-
Country/ Type of e-waste Reference wastes has also drawn the attention of various researchers who have
Organization been actively involved in this field and are continuously publishing
European Union (1) Temperature exchange European Union numerous research articles and reviews every year. However, most of
(EU) equipment, (2) Screens and monitors, (2018) the reviews on e-wastes recycling are largely restricted to policies and
(3) Lamps, (4) Large equipment legislations to promote the recycling of metallic fractions from e-wastes
(dimension >50 cm), (5) Small (Kumar et al., 2017), to evaluate their effect on humans (Awasthi et al.,
equipment (dimension ≤50 cm), and
(6) Small IT and telecommunication
2016), environment (Yang et al., 2020) and on the economy (Ravindra
equipment (dimension ≤50 cm). and Mor, 2019). Other reviews available in this field include feasibility
China (1) Refrigerator, (2) Monitors and Forti et al. (2018) studies of various pretreatment stages of recycling (Duan et al., 2011),
TVs (3) Washing machine, (4) Air current recycling trends & challenges (Tabelin et al., 2021) and metal
conditioner, (5) Water-heater, (6)
specific recycling techniques such as precious metals (Lu and Xu, 2016)
Personal computer (7) Fax and
telephone machine, (8) Mobile or rare earth metals (Sethurajan et al., 2019) recovery methods from
phone, (9) Printer, and (10) Copier. e-wastes. Reviews on specific metal recovery processes such as hydro­
United Nations (1) Central heating, (2) Photovoltaic Forti et al. (2018) metallurgy (Cui and Anderson, 2016; Li et al., 2018), biometallurgy
University panels, (3) Professional heating & (Işıldar et al., 2018; Desmarais et al., 2020), supercritical fluid extrac­
(UNU) ventilation, (4) Dishwashers, (5)
Kitchen equipment, (6) Washing
tion (Li and Xu, 2019) and ionic liquid extraction techniques (Schaeffer
machines, (7) Dryers, (8) Household et al., 2018) can also be found. Limited review articles were found that
heating & ventilation, (9) Fridges, focused on the overall metal recovery techniques (Zhang and Xu, 2016;
(10) Freezers, (11) Air conditioners, Chauhan et al., 2018); however a thorough comparison and analysis is
(12) Other cooling equipment, (13)
still lacking for these methods. Thus, to address the knowledge gap, an
Professional cooling equipment, (14)
Microwaves, (15) Other small attempt has been made to provide a comprehensive review on different
household equipment, (16) pre-treatment and metal recovery techniques from e-wastes as well as
Equipment for food preparation, (17) the advancements made in these techniques. Further, critical evaluation
Small household equipment for hot of different metal recovery techniques has been done based on the
water preparation, (18) Vacuum
available life cycle assessment (LCA), techno-economic, and
cleaners, (19) Personal care
equipment, (20) Small IT equipment, industrial-scale studies to identify the possible limitations in the pub­
(21) Desktop PCs (excluding lished processes. Finally, perspectives and analysis of different recovery
monitors, accessories), (22) Laptops, methods with critical discussion have been presented to suggest poten­
(23) Printers, (24)
tial directions for future research towards the development of a more
Telecommunication equipment, (25)
Mobile phones, (26) Professional IT sustainable way of metal recovery techniques from e-wastes.
equipment, (27) CRT monitors, (28)
Flat display panel monitors, (29) 2. Methodology for literature survey
Small consumer electronics, (30)
Portable audio & video, (31) Music
Instruments, radio & Hi-Fi, (32)
A three-step investigative methodology was followed for reviewing
Video & projectors, (33) Speakers, the different metal recovery techniques from e-wastes. At first, a thor­
(34) Cameras, (35) CRT TVs, (36) Flat ough search of peer-reviewed articles, reports, book chapters, etc. was
display panel TVs, (37) Small lighting done on different web sources, viz. Google Scholar, and Science Direct
equipment, (38) Compact fluorescent
using keywords such as “e-waste” & “metals”, “WPCB” & “recycle”,
lamps, (39) Straight tube fluorescent
lamps, (40) Special lamps, (41) LED “recover” & “metallurgical technique”, and so forth. Then, recent studies
lamps, (42) Household luminaires, published in reputed journals between 2010 and 2021 were selected and
(43) Professional luminaires, (44) sorted in time sequence. Only relevant articles falling within the scope of
Household tools, (45) Professional the present study were reviewed after screening the abstracts of the
tools, (46) Toys, (47) Game consoles,
(48) Leisure equipment, (49)
papers. This was followed by classification of different conventional and
Household medical equipment, (50) novel metal extraction techniques. Representative examples from each
Professional medical equipment, (51) of these techniques were selected based on the objective, concept,
Household monitoring & control methods and results of the experiments for further summarization and
equipment, (52) Professional
review of the process. Finally, critical evaluation and comparative
monitoring & control equipment,
(53) Non-cooled dispensers, and (54) analysis of different metal recovery technologies were carried out to
Cooled dispensers. identify the perspectives and scope for future research in the relevant
India (1) Information technology and MoEF&CC (2016) field.
telecommunication equipment
(computer, laptop, notepad, printers,
copying equipment, telephone,
3. Pre-treatment methods
cellular phones, etc.), and (2)
Consumer electrical and electronics The heterogeneous nature and complicated structures of e-wastes
(television, refrigerator, washing make it difficult to find a suitable and specific recycling technique. In
machine, air conditioner, fluorescent
addition, the presence of hazardous substances makes the recovery
and other mercury containing lamps).
Japan (1) Large home appliances (air Ministry of the process even more complex. Therefore, pre-treatment of these wastes is
conditioners, TVs, refrigerators, Environment of required which plays an important role in overcoming these difficulties
washing machines and dryers), and Japan (2014) to a greater extent. The different pretreatment methods involved during
(2) Small home appliances (PCs, the recovery process aid in enriching the metallic concentration in the
mobile phones, digital cameras,
clocks, hair dryers, etc.).
output stream by enhancing the separation efficiency of the metallic and
non-metallic fractions (NMFs) (Marra et al., 2018). Different
pre-treatment stages of e-wastes are shown in Fig. 2 which are further
reviewed in detail in the following sub-sections.

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R. Kumari and S.R. Samadder Journal of Environmental Management 320 (2022) 115887

3.1. Disassembly 100% for surface mounted components (SMCs) and pin through hole
components (PTHCs) under optimal temperature and incubation period
Disassembly is the first step involved in the recycling process of the e- of 260 ◦ C and 2 min respectively. But, the disassembly rate for other
wastes. There are certain reusable and hazardous components such as small SMCs (>3 mm) was 40–50% lower than these SMCs and PTHCs.
socket pedestal, screw joints, cathode ray tubes (CRTs), batteries, ca­ Further, Wang et al. (2016) designed a pilot-scale automatic disassembly
pacitors, and electronic chips found attached with these wastes that are unit with an off-gas purification system. The disassembly unit success­
required to be treated differently (Duan et al., 2011; Kumar et al., fully dislodged SMCs from WPCBs except certain small PTHCs within 8
2020b). During the disassembly stage, all these components are sys­ min of the incubation time. Marconi et al. (2019) developed a prototype
tematically removed to prevent their entry into the mainstream of the of automatic disassembly system comprising a wave soldering machine,
recovery process. This step of pre-processing can be accomplished either a manipulator equipped with vacuum gripper for components picking,
in selective or simultaneous way. The selective type of disassembly is and a central control unit for co-ordination. Each SMC is exposed to high
based on the principle of ‘look and pick’ where, the connections and temperatures within the unit for a limited duration that resulted in
joints in e-wastes are identified first, followed by the individual disas­ effective detachment of components without any damage. Also, a proj­
sembly of the components. While, the simultaneous dismantling which ect (ADIR) was launched by European consortium for disassembling
is based on the principle of ‘evacuate and sort’ is usually applied in case mobile phones and other PCBs’ components. The disassembling tech­
of printed circuit boards (PCBs) where, all the components are removed nique involved various measurements of the PCBs using 2D and 3D laser
simultaneously by heating the whole board in the furnace. Although, images to mark components with potentially high amounts of valuable
simultaneous disassembly has higher efficiency; however, it enhances material, such as tantalum. These data are then used to extract co­
the processing time, cost, and the risk of damaging the components ordinates for the laser beam control to selectively cut out parts or to
during heating (Chauhan et al., 2018). unsolder SMCs of PCB with an average cutting speed of 50 cm/min for
Currently, the informal practice of manual disassembly is more each board (Noll et al., 2018).
common in developing countries; while mechanical disassembly is Automatic dismantling equipment being expensive is ideally suitable
frequently practiced by developed nations. Manual dismantling in­ for e-wastes with high metal contents. However, manual dismantling is
corporates the use of hammers, chisels, cutting torches, etc. to separate still the most common disassembly method practiced in most of the
the components and to open the solder connections. The method also recycling centers of developing nations. Therefore, an appropriate
often employs open burning and heating of the e-wastes for further disassembly method should be chosen depending on the quantity and
separation of the components which are detrimental to the human quality of metallic fractions available in the waste stream in order to
health and the environment. High labor cost, more material wastage, reduce the recovery cost and to enhance the recovery efficiency.
and environmental & health hazards associated with the informal
practices restricted their application and popularized the mechanical
3.2. Size reduction
means of dismantling practices in the developed nations (Hsu et al.,
2019). Mechanical dismantling is either semi-automatic or automatic.
After dismantling and sorting of the reusable and hazardous ECs
The semi-automatic method uses the external forces such as shearing or
vibration along with the heating system for liberation of the attached from e-wastes, the remaining wastes undergo different mechanical
components from e-wastes. The fully automatic mechanical method is processing of size reduction such as shredding, crushing, and grinding
designed to separate the reusable and hazardous components from the for effective separation of metallic and NMFs. This comminution is also
waste stream. In recent years, several researchers have worked on the required for super-capacitors to strip the activated carbon off the
development of greener and automatic dismantling methods of e-wastes. aluminium foil before undergoing other pre-treatment methods (Kumar
For example, Park et al. (2015) developed a disassembly unit with and Kim, 2018; Pallavolu et al., 2021). Different mechanical instruments
infrared heat treatment facility for separating electrical components such as hammer crushers, disc crushers, granulators, rotary crushers,
(ECs) from waste PCBs (WPCBs) with 94% separation efficiency. Chen shredders, and cutters are used for reducing the size of e-wastes. The
et al. (2013) used combinations of hot air treatment and mechanical selection of the equipment is usually based on the strength, hardness,
vibration as dismantling method. The disassembly rate reached almost particle size, and other properties of the components of e-wastes (Yang
and Xu, 2011). Normally, hammer crushers with high shearing and

Fig. 1. Composition of e-wastes.

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impact forces are suitable and sufficient enough to comminute the 3.4. Enrichment
e-wastes but ball milling and disc milling are also often employed for
further pulverization (Ghosh et al., 2015). This pulverization is required After screening and sieving, the ground particles undergo different
for achieving a higher degree of liberation for enhancing the metal re­ physical treatment methods. Physical recycling is done primarily to
covery efficiency. Arshadi et al. (2018) analyzed the effect of particle enrich the metal contents by separating NMFs from the remnants of e-
size distribution on metal recovery efficiency and found that the wastes. The methods involved in the physical treatment segregate the
maximum extraction efficiencies for Cu, Ag, Ni, and Ti were achieved for metallic and NMFs on the basis of differences in various physical char­
finer particles (<1 mm) of e-wastes. No interlocking between metallic acteristics of the materials (Yang and Xu, 2011). Degree of separation
and NMFs was reported after milling e-wastes to below 150 μm size. and efficacy of the method depend on the shape, size, and distribution of
Recently, Zhou et al. (2016) studied the effect of cryogenic grinding in the particles (Ghosh et al., 2015). A summary of different physical
size reduction of WPCBs. The decreased temperature favored the size separation and enrichment methods is given in Table S1 which is further
reduction (0.5–1.4 mm) with minimal power consumption than con­ reviewed in following sub-sections. The separated metallic fractions
ventional crushing techniques. after enrichment undergo different refining and purification processes
Although comminution of e-wastes is necessary for effective sepa­ for recovery of the individual element.
ration, there are certain challenges associated with this process. The
generation of fine dust during crushing and pulverization of e-wastes is 3.4.1. Air separation
one of the major issues (Ghosh et al., 2015). Also, the energy demand Air classification method is used to separate metallic and NMFs of
and subsequent cost hikes affect the overall efficiency of the recovery different sizes based on density of different components of the pulver­
process. Further, the excessive crushing results in agglomeration of the ized e-wastes mixture. The principle of separation is based on the dif­
polymeric fraction and loss of metallic fractions; while inadequate ference in their terminal settling velocity (Vt). The heavier particles with
comminution deteriorates the quality and degree of liberation of mate­ larger Vt move downwards against the air stream at shorter distance;
rials from e-wastes (Ruan and Xu, 2016). while the lighter particles rise on the top of the column along with the air
stream and settles at larger distance (Eswaraiah and Soni, 2015).
3.3. Screening and sieving The air current separation method involves the use of different types
of air classifiers. For example, Zhou et al. (2016) successfully applied air
The size and the properties of metallic fractions are different from table for separation of grade materials in the range of 0.5–2.8 mm from
that of NMFs. This variation in the size of particles necessitates per­ WPCBs. Ribeiro et al. (2019) used zig-zag air classifier to separate lighter
forming the screening and sieving of these wastes for further classifi­ fractions from heterogeneous powdered mixture of e-wastes. The sepa­
cation and recovery. Screening is usually performed for relatively ration enhanced the Cu content from 13.8% to 48.8% in the pulverized
coarser materials, as the efficiency reduces for finer materials (Ardente WPCBs. In other studies, fluidized bed separators have also been used as
et al., 2014). This step assists in preparing a uniform feed size and in physical air separation method. Zhang et al. (2017a) utilized vibrating
upgrading the metal contents. Different types of screening equipment of gas-solid fluidized bed separator for segregating metallic and NMFs;
stationary and rotating types are used in recycling industries; however, however, the separator showed poor segregation efficiency for fine
the primary method of screening is usually done using rotating screen or particles (<0.25 mm). Stronger interactive forces among these
trommel. These large drum-shaped trommel screens mainly separate finer-sized particles resulted in their agglomeration, thereby reducing
coarser substances from bulk material. Sieves of different sizes are used their segregation efficiency. Moreover, the separation efficiency was
for classification of different-size materials. The screening is generally found to be dependent on the shape, size, & density of the components
limited to the particle size of about 250 mm; while the finer particles along with the superficial air flow rates, fluidization time and fluidiza­
below this size undergo the process of classification (Kaya, 2016). The tion frequency. Barnwal and Dhawan (2019) compared the air and
size sorting and classification of particles are necessary for enhancing water-based fluidization processes where, the air fluidization process
the efficiency of different physical separation methods. Kumar et al. yielded higher weight efficiency and metal recovery than the water
(2013) found that the separation efficiency was enhanced up to 90% fluidization technique. Although these methods have certain advantages
after sorting particles based on different size classifications for WPCBs of in terms of their simpler operation and lower energy consumption, the
DVDs. Similarly, Bilesan et al. (2021) revealed the feasibility of using common problems associated with this method are the low-quality
sieving for recovering precious metals as sieving separated the product, added workload, and difficulty in further refining. Besides,
maximum Au fraction in the finer classification (<75 μm) and Cu in the successive grinding and milling are required in certain air separators for
coarser fractions. The size classified fractions are then sorted based on higher metal liberation (Kaya, 2018).
their density, conductivity, and other physical parameters.

Table 2
Weight composition of metals and their economic value distribution in different types of e-wastes.
Type of e- Metal content (% by weight) and economic value distribution (%) (in brackets) Reference
wastes
Cu Fe Si Sn Al Zn Pb Co Mn Ni Ag Au

Computer PCBs 36.14 0.53 4.19 2.14 5.96 2.06 1.45 - (0.00) 0.03 0.09 0.03 _ Arshadi et al.
with wire (73.00) (− ) (2.30) (12.70) (3.60) (2.00) (1.10) (0.02) (0.29) (4.90) (2018)
Mobile phone 57.47 25.23 8.8 3.49 0.77 4.29 0.85 0.23 0.24 5.10 0.15 0.12 Fontana
(5.52) (0.47) (2.18) (0.98) (0.02) (0.20) (0.03) (0.25) (0.01) (0.82) (1.34) (88.01) et al. (2019)
Television PCBs 14.4 5.00 2.15 3.61 4.14 2.06 2.18 - (0.00) 0.06 0.24 0.04 _ Arshadi et al.
(44.58) (− ) (1.79) (32.58) (3.84) (3.00) (2.46) (0.05) (1.24) (10.38) (2018)
Waste DVD 17.8 5.51 3.79 2.57 10.10 1.99 3.33 0.04 0.24 0.36 – _ Kumar et al.
(52.88) (3.15) (3.04) (22.34) (9.02) (2.79) (3.62) (1.17) (0.19) (1.79) (2013)
CPU 30.51 9.44 9.56 1.80 5.10 0.26 0.82 0.39 0.06 3.61 0.13 _ Arshadi et al.
(50.52) (− ) (4.27) (8.71) (2.54) (0.20) (0.50) (6.34) (0.03) (9.9) (16.83) (2018)
Fax machine 21.03 6.56 8.82 3.04 6.14 1.26 1.77 - (0.00) 0.51 0.57 0.14 _ Arshadi et al.
(44.32) (− ) (5.02) (18.75) (3.89) (1.26) (1.36) (0.29) (2.00) (23.07) (2018)
Refrigerator 3.4 50 – – 1.1 – – – – – – _ Zeng et al.
(25.5) (72.1) (2.48) (2016)

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R. Kumari and S.R. Samadder Journal of Environmental Management 320 (2022) 115887

Fig. 2. Pre-treatment methods of e-wastes.

3.4.2. Gravity separation process of e-wastes. The crushed particles of e-wastes often contain a
Gravity separation method is a density-based separation process relatively larger content of iron and nickel than other metals. These
employed for separating lighter fractions from heavier fractions. The metals possess magnetic properties that can be used for their effective
comminuted particles of e-wastes constitute a diverse range of metallic separation from the rest of the materials. Thus, magnetic separators
and NMFs with varying specific gravity. This difference in specific exploit the difference in the magnetic properties of comminuted e-
gravity is utilized by the gravity separators where, the fractions with wastes particles to separate the ferrous and non-ferrous components
higher specific gravity get separated from lighter fractions by the rela­ (Lim et al., 2014).
tive movement of heavier fractions in response to gravity. The forces Magnetic separators, specifically low-intensity drum separators are
exerted by denser liquids and size & shape of the particles also play an used for separating ferromagnetic components from non-ferrous com­
important role in separating metallic fractions (Kaya, 2016). ponents. These low-intensity magnetic separators are more efficient in
Various types of equipment such as water tables, hydro-cyclones, recovering the coarser and strongly magnetic materials only; thus, a
jigs, rising-current separators, Falcon centrifugal separators, etc. have high-intensity magnetic separator (HIMS) is required for recovering the
been used so far as gravity separators in e-wastes recycling. Different paramagnetic materials (Bentli et al., 2017). Much advancement in
dense liquid media such as tetrabromoethane and acetone have also design and operation of HIMS has been achieved for enhancing the
been used in the sink-float method of gravity separation to separate the separation efficiency of the process. These separators have a conveyor
metals from NMFs of comminuted e-wastes. The separated lighter frac­ belt where, the magnetic substances get attracted while, the non-ferrous
tion floats on the surface while, the heavier fraction settles at the bot­ materials fall freely into the collection tank under the gravitational in­
tom. Rodrigues et al. (2021) used sodium silicate as a dense liquid fluence (Ruan and Xu, 2016). The method, thus, aids in enriching the
medium to enrich the metallic content in the WPCBs. The contents of Cu, ferromagnetic content in the output fraction. Fujita et al. (2014) carried
Ag, and Au in the remnant enhanced by 17.37%, 0.74%, and 0.22% out the magnetic separation of WPCBs at a lower magnetic field strength
respectively after the dense medium separation. In another study, Sarvar and found that the nickel content in the magnetic product was enhanced
et al. (2015) recovered up to 97.5% of the metallic constituents from a from 0.16% to 6.7%. Ruan and Xu (2016) found that the recovery rate of
coarser fraction (0.59–1.68 mm) of WPCBs using wet jigging process. iron particles from crushed waste refrigerator cabinets and toner car­
Tanısalı et al. (2021) studied the effect of gravity separation on bene­ tridges reached almost 99% after magnetic separation. One of the major
ficiation of comminuted WPCBs and metal recovery efficiencies and issues associated with this method is the agglomeration of the ferrous
revealed that the recovery efficiencies for different metallic fractions and non-ferrous particles that further attract other non-ferrous mate­
(96.8% for Au, 96.7% for Ag, and 97.7% for Cu) were enhanced in the rials. Another issue is its inefficiency to separate individual metals from
heavier fraction. These different methods of gravity separation are their alloys (Hadi et al., 2015). Besides, they have poor separation ef­
usually adapted as a cleaner approach to recycle and enrich the metallic ficiency for the dust obtained during PCB comminution. Recently,
elements in the left-out fraction. Oluokun and Otunniyi (2020) proposed chemical conditioning of the
dust using octyl phenol ethoxylate as a solution to combat these effects.
3.4.3. Magnetic separation Efficient wet magnetic separation was obtained for PCB dust particles of
Magnetic separation method has been widely used in pre-treatment size 150–212 μm with 97% and 94% recovery efficiencies for Fe and Ni

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R. Kumari and S.R. Samadder Journal of Environmental Management 320 (2022) 115887

respectively. electrostatic separation process is poor for smaller particle sizes.

3.4.4. Electrostatic separation 3.4.5. Froth flotation


Electrostatic separation is another pre-treatment method that sepa­ Natural hydrophobicity of plastics and other NMFs has been exten­
rates the conductive and non-conductive materials of e-wastes on the sively utilized in the processing of e-wastes. It has been found that even
basis of their conductivity or resistivity differences (Ruan and Xu, 2011). reagent-free flotation of the coarser fraction of e-wastes yields an
The electric field generated by the conductive or metallic fraction is excellent recovery with a good quality product. Mäkinen et al. (2015)
utilized to separate them from the less conductive or NMFs. This capa­ revealed that a relatively large amount of Cu, Ni, Pb, and Sb can be
bility of separation is dependent on the amount of charge acquired and found in the froth even without the use of any reagents. However, the
the difference in polarity between the particles of comminuted e-wastes addition of frother such as bromoform and benzene helps in stabilizing
(Matsusaka et al., 2010). the froth and in enhancing the kinetics. Flotation using water and air has
There are three different techniques under electrostatic separation also been introduced as green floatation technique for recycling WPCBs
which are usually used for separating conductive and non-conductive (Estrada-Ruiz et al., 2016). Further, Zhu et al. (2020) studied the
materials. These methods typically include corona electrostatic separa­ dissociation and flotation behaviors of different sized particles of WPCBs
tion (CES), eddy current separation (ECS), and triboelectric separation and revealed that the distribution rate of the particles increased with the
(TES). The CES or the induction charging technique effectively separates reduction in particle size. Also, it was found that Au and other base
the metallic and NMFs that possess significant differences in their den­ metals can be successfully recovered by flotation using kerosene from
sity and conductivity. Catinean et al. (2021) demonstrated that the CES the shredder light fractions (Jeon et al., 2018). Thus this method can be
method is efficient enough to recover up to 95% of Cu from a fine widely used for separation of fine particles from e-wastes. Froth flotation
polyvinyl chloride (PVC) and Cu granular mixture of low metal content has certain advantages including high efficiency for a large range of
(less than 15%). Similarly, the ECS method is also useful in separating particle size, lower dust emission, and more economical; however, it
ferrous and non-ferrous metals. The separation technique is dependent often requires treatment for the residual water (Ruan and Xu, 2016).
on the gravitational, centrifugal, frictional, and magnetic deflection
forces for the separation of ferrous materials. However, the magnetic 4. Metal recovery techniques
deflection force is the pre-dominant force responsible for the separation
(Jujun et al., 2014). In recent years, researchers have further explored After pre-treatment of e-wastes, further processing is required to
the ECS method with rotating electrodes or pulsed excitation and on obtain enriched and pure metallic fractions. Various metallurgical as
optimization of specific operating conditions for efficiency enhancement well as other novel techniques have been employed so far after the
of the method (Li et al., 2017). disassembly and separation of metallic and NMFs of e-wastes. Fig. 3
Tribo-electricity or contact charging technique is useful for charging depicts the different approaches employed for extracting metals from e-
and separating the materials with similar conductivities. The difference wastes and the same has been reviewed in detail in the following
in triboelectric charge between the organic and inorganic materials is sections.
used to separate the inorganic materials from NMFs of e-wastes (Zhang
et al., 2017b). Zhang et al. (2018b) found that TES technique
strengthens the gravity separation process resulting in enhanced metal 4.1. Pyrometallurgical process
recovery from 76.39% to 81.41%. However, the overall efficiency of the
Pyrometallurgical process is a traditional approach of metal recovery

Fig. 3. Different methods of metal recovery from e-wastes.

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R. Kumari and S.R. Samadder Journal of Environmental Management 320 (2022) 115887

where, different thermal treatments such as incineration, roasting, sin­ extraction methods. Calderon et al. (2020) utilized magnetic nickelif­
tering, and smelting are carried out under controlled high-temperature erous pyrrhotite, a mined-waste product as an adsorbent to recover Au
to recover the metallic components from e-wastes. The heating is usu­ from chloride solutions. Further, alternative approaches such as
ally done in specialized incinerators, blast furnaces, or plasma arc fur­ enhanced cementation and coupled magnetic separation-cementation
naces where, the crushed scraps containing metals are volatilized under methods are also explored to overcome the limitations of these pro­
high temperature and the impurities are converted into slags to obtain cesses and to enhance the recovery efficiency (Jeon et al., 2020).
coarse metal ingot (Zhang and Xu, 2016). Also, thermal desoldering of Recently, Choi et al. (2021) revealed that the enhanced cementation
e-wastes is usually done using electric heating tubes, infrared heating, technique using Al and activated carbon (AC) together increased the
liquid heating media including dielectric liquids and molten salts (Kaya, overall recovery efficiencies of Cd2+, Zn2+, Ni2+, and Co2+ in compar­
2018). ison of using Al or AC individually. Similarly, Jeon et al. (2021)
Thorough reviews have been carried out on various pyrometallur­ enhanced the Au recovery from ammonium thiosulfate using galvanic
gical recovery routes such as Noranda smelting process, Aurubis smelter, interactions between Al and AC.
Umicore’s Smelter, and Boliden Ronnskar Smelter for different metals
by Ebin and Isik (2016) and Wang et al. (2017). These methods are 4.2.1. Traditional inorganic acid leaching method
currently being practiced worldwide for processing the metallic frac­ Traditional leaching methods using various inorganic acids such as
tions of e-wastes; however, high investment cost and energy demand HCl, HNO3, H2SO4, and their combinations have been well investigated
along with the release of toxic fumes are some of the major limitations of for selective and non-selective extraction of metals from e-wastes. Aqua
these pyrometallurgical techniques. regia, a combination of nitric acid and hydrochloric acid (HCl:HNO3 =
In recent years, researchers have investigated the potential of low 3:1, v/v) has also been extensively used for non-selective and aggressive
temperature roasting in presence of different chlorinating agents. Panda digestion and solubilization of precious and base metals of e-wastes
et al. (2020) performed low temperature roasting of WPCBs in presence (Cyganowski et al., 2017). These acids, when used alone, are also
of NH4Cl and recovered about 93% Cu and 100% Pb, Ni, and Zn under capable of selectively extracting metals from the metallic mixture.
optimized roasting conditions (temperature: 300 ◦ C, time: 4 h, and Hossain et al. (2018) reported that the maximum Cu extraction from
NH4Cl dose: 3 g/g). Studies on combination of pyrometallurgical tech­ WPCBs reached 190 mg/g within 60 min of the selective extraction
niques and other metal recovery techniques have also been explored to using concentrated H2SO4. Innocenzi et al. (2017) designed a mobile
enhance the metal recovery efficiency while, averting environmental plant under HydroWEEE-demo project for the treatment of e-wastes
impacts. Jadhao et al. (2020) employed an integrated technique of based on the selective extraction using inorganic acid leaching system.
mild-temperature pyrolysis and ultrasonication for simultaneous re­ The recovered products showed leaching efficiencies of around 90% for
covery and recycling of the metallic and polymeric fractions to produce Cu, Au, Ag (PCB), 95% for Y and Eu (lamp and CRT powders), 93% for
fuel-grade gases. Approximately 90 wt% of metallic fraction was Li, and >97% for Co (Li-ion battery).
recovered within 30 min of the process. Also, attempts have been made Generally, the base metals including Al, Fe, Zn, and Sn can be easily
to transform the WPCBs into value-added metallic alloys instead of solubilized in dilute acids; however, leaching of Cu requires either an
producing pure metals using pyrometallurgical techniques (Shokri et al., oxidizing acid or a non-oxidizing agent with an oxidant for efficient
2017). dissolution. Birloaga et al. (2014) studied the H2SO4 leaching procedure
with hydrogen peroxide (H2O2) as an oxidant for Cu extraction from
4.2. Hydrometallurgical process WPCBs. Three-step oxidative leaching procedure was required to ach­
ieve maximum Cu extraction efficiency (99%). Somasundaram et al.
Hydrometallurgical technique is usually considered as a more exact, (2014) used 0.1 M CuCl2 as an oxidant in HCl leaching system for se­
highly flexible, predictable, and easily controllable method for metal lective extraction of Sn (92%) from WPCBs and further revealed that
extraction from e-wastes. The process involves two essential stages, viz., leaching of Cu, Pb, and Ni is feasible with an elevated CuCl2 concen­
extraction stage for solubilization of metals using suitable lixiviants and tration of 0.5 M.
refining stage for recovery of leached metals from the polymetallic The concentration of these inorganic acids is the most influential
pregnant leaching solution (Silvas et al., 2015). Many leaching agents parameter in determining the efficiency of the process. Bas et al. (2014)
such as aqua regia (Cyganowski et al., 2017), inorganic acid (Yazici and revealed that the extractions can be enhanced from 88.5% to 99.9% and
Deveci, 2014), cyanide (Bisceglie et al., 2017), halide (Altansukh et al., 14%–68% for Cu and Ag respectively with the increase in concentration
2016), thiourea (Birloaga et al., 2014), thiosulfate (Jeon et al., 2019), of nitric acid from 1 to 5 M. Similar results were obtained in the study
and ammonia (Xiao et al., 2013) have been used for extraction of conducted by Ajiboye et al. (2019) where, the leaching efficiency of Cu
different base, precious, critical, and rare earth elements from e-wastes. increased from 52.7% to almost 100% with an increase in concentration
These leaching systems are considered less hazardous than pyrometal­ of HNO3 from 0.25 M to 1.0 M. Apart from the concentration of the
lurgical process except for certain lixiviants like cyanide, aqua regia and acids, temperature, pH, solid to liquid (S/L) ratio, and size of e-waste
other mineral acids. A slow leaching kinetic and generation of volumi­ sample are some of the other predominant parameters which affect the
nous liquid wastes and sludge are some of the other concerns associated rate of leaching process (Jha et al., 2012). Variation in these parameters
with the process. The different leaching systems with their advantages influences the mass transfer coefficient, flux of H+ ions and diffusivity
and disadvantages have been further discussed in the following across the particle boundaries which in turn influence the rate of reac­
sub-sections. Also, summary and critical evaluations of these leaching tion (Kumari et al., 2016).
systems along with their efficiency under different optimal conditions Studies have revealed that inorganic acids can effectively extract
have been presented in Table S2. different base metals from e-wastes under relatively moderate condi­
After extraction, the recovery of these metals is generally done using tions, but requirements of higher concentrations of acid, oxidant,
adsorption, solvent extraction, cementation using Zn, Al, Ni, & Fe and leaching time, temperature, and pressure make the process uneconom­
electrowinning methods (Kumar et al., 2020a). Selection of these ical. Besides, the volatile nature of acids and the potential release of
methods is dependent on the leaching system used for metal extraction, toxic gases such as NOx from these inorganic acids possess potential risks
content of target metals and amount of impurities present in the leaching for workers and the environment. Corrosive nature of mineral acids,
solution. For example, the maximum recovery of precious metals from large amount of acid waste, and unwanted by-products are some of the
acidic thiourea and other thio leaching systems has been achieved using other concerns associated with the inorganic acids leaching system (Li
cementation method; while, the recovery of other metals such as Cu, Co, et al., 2018).
& Ni is generally done using conventional electrowinning and solvent

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R. Kumari and S.R. Samadder Journal of Environmental Management 320 (2022) 115887

4.2.2. Cyanide leaching method This ammonia-ammonium leaching system has also shown leachability
Cyanide leaching for precious metal extraction from e-wastes has for other base metals depending on the reduction potential of metals and
been extensively studied by various researchers (Petter et al., 2014; stability of the metal-ammine complex (Xiao et al., 2013).
Bisceglie et al., 2017). The lixiviant is preferably used for recovery of Ag In recent years, different halide leaching systems such as chlorine-
and Au from mines because, of its higher efficiency and lower cost chloride (Yazici and Deveci, 2015), and iodine-iodide (Altansukh
involvement. However, the cyanide leaching of e-wastes is avoided due et al., 2016) leaching systems have been used for precious metals
to its high toxicity (Akcil et al., 2015). extraction under alkaline environment. Pereira et al. (2020) found an
Cyanide ions (CN− ) can be found as complexes, hydrogen cyanide extraction efficiency of 96% for Ag when WPCBs of computers were
(HCN), free cyanide ions (CN− ), or simple compounds in solutions leached using the combination of sodium chloride and calcium hypo­
depending on pH. However, cyanidation at pH ≥ 10.5 is considered as chlorite. Xiu et al. (2015) reported an enhancement in the extraction
economical and eco-friendly because of the limited formation and efficiency of iodine–iodide leaching system for Au, Ag, and Pd after
volatilization of toxic HCN. Besides toxicity, the presence of large supercritical water oxidation (SCWO) pre-treatment of WPCBs. Envir­
amount of Cu in WPCBs results in excessive consumption of cyanide oLeach Technologies Inc. in Canada has patented a process based on the
which in turn increases the cost considerably. One of the ways to iodide-iodate and electrolysis method for precious metals recovery from
overcome such a problem is to introduce a multi-stage leaching system e-wastes with reagent recycling system (Nelson et al., 2017). The
where the base metals are extracted at the first stage followed by non-toxic and non-corrosive nature of this leaching system together with
precious metals extraction at the second stage. Another way to reduce its fast kinetics and good selectivity for precious metals make it an
cyanide consumption during leaching process is the addition of other appropriate leaching solution for precious metal extraction. Also, the
lixiviants that can combine with cyanide to form complexes with metals. complex formed between Au-iodide is a very stable compound. Never­
Preliminary research conducted by Bisceglie et al. (2017) revealed that theless, high reagent consumption and cost of iodine are some of the
3-nitrobenzene-sulphonate (NBS) can improve Au recovery rate from major limitations associated with this leaching system (Ghosh et al.,
e-wastes. 2015).
Sufficient information on toxicity and safe handling of cyanide (In­
ternational Cyanide Management Code) is available; however, the 4.2.4. Organic solvent etching method
practice of cyanide leaching at the industrial level is still not feasible In recent years, some organic acids such as citric acid (Li et al.,
because of high toxicity and environmental consequences associated 2010), oxalic acid (Cui et al., 2019), and acetic acid (Natarajan et al.,
with the leaching system. Moreover, the chances of leaching of residual 2018) have been introduced as environment-friendly lixiviants for
cyanide from effluents (if not treated properly) into the soil and extraction of metals from e-wastes. Chen et al. (2015b) proposed a green
groundwater are very high which will result in chronic health problems. method for sustainable extraction of Co and Li from spent Li-ion batte­
Therefore, the focus of the research on precious metal leaching from e- ries using citric acid as the major lixiviant in combination with other
wastes has been shifted towards the development of a less toxic and different reductants (Tea Waste, Phytolacca americana branches, and
much milder leaching system. hydrogen peroxide). The leaching results revealed better efficiencies for
the combinations of citric acid & tea-waste (96% for Co and 98% for Li)
4.2.3. Mild leaching method and of citric acid & H2O2 leaching system (98% for Co and 99% for Li)
Several mild leaching agents such as ammonia-ammonium (Sun under optimized conditions. In another study, Varshney et al. (2017)
et al., 2015), halide (He and Xu, 2015; Patel and Dawson, 2015), and used DL-malic acid and H2O2 as leaching agents that resulted in more
thio-based lixiviants, viz. thiosulfate (Jeon et al., 2018), and thiourea than 90% extraction of Cd, Pb, and Ni from WPCBs.
(Birloaga and Vegliò, 2016) have also been investigated. Amongst these Besides, glycine (amino acid) has also been used as organic lixiviant
leaching agents, the thio-based and halide leaching agents are mainly with different oxidants (O2, H2O2, and Cu2+) and catalysts/synergists for
used for precious metals extraction; while the ammonia-ammonium effective extraction of precious and base metals from e-wastes. Oraby
leaching agent is used mainly for extraction of base metals. et al. (2020) used glycine as a lixiviant in an alkaline environment for
Thio-based leaching system has been seen as a promising substitute precious and base metals extraction from WPCBs with leaching effi­
of cyanide leaching system for precious metals owing to its low corro­ ciencies of 92.1%, 85.3%, 98.5%, 89.8%, and 99.1% for Au, Ag, Zn, Pb,
sivity, high selectivity, and reduced environmental risk. Jing-ying et al. and Cu respectively. Similarly, Li et al. (2020) developed a sustainable
(2012) extracted 90% Ag from WPCBs using thiourea within 2 h of the approach for extraction of Cu from WPCBs using alkaline glycine solu­
leaching process. In another study, Birloaga and Vegliò (2016) followed tion in which, a maximum Cu extraction of 96.5% was achieved together
a two-step leaching process using H2SO4 and H2O2 in the first step for with high co-extraction of other base metals.
base metals extraction and acidic thiourea in the second step for
precious metals extraction (Ag-75%; Au-90%). Gámez et al. (2019) 4.3. Biometallurgical process
proposed a feasible leaching system using ammonia-thiosulfate solution
and ion exchange resin method for extraction and recovery of precious Bio-metallurgical processing of e-wastes is an emerging eco-friendly
metals from WPCBs. This method can recover more than 80% of the metal recovery technique that has attracted much attention of the re­
precious metals (Ag and Au). Similarly, Jeon et al. (2019) enhanced searchers for making practical application of the process. It is the process
(around 15-fold) Au extraction from waste mobiles using ammonium that involves utilization of metal-microbe interactions during bio­
thiosulfate solution after pre-treatment with different physical separa­ leaching and biosorption stage for metal extraction and their subsequent
tion methods. A non-cyanide based alternative method has also been recovery from e-wastes (Awasthi et al., 2019). Tables S3 and S4 present
developed by Uwin Nanotech of Taiwan which is operational at indus­ a detailed critical evaluation of the various bioleachants and biosorbents
trial level for precious metals recovery with around 99% product purity used for metal extraction and recovery from different e-wastes.
(UWin Nanotech, 2019). Chemo-lithoautotrophic bacteria such as Acidithiobacillus ferroox­
Ammonia-ammonium leaching is another suitable lixiviant for se­ idans and Acidithiobacillus thiooxidans are the group of microorganisms
lective extraction of Cu from e-wastes. Sun et al. (2015) investigated the that have been considered the most for bioleaching of the elements
ammonia-ammonium carbonate leaching system for Cu extraction from available in e-wastes. Other heterotrophic bacteria and fungi are also
e-waste mixture and reported high Cu recovery (>90%) and high being used in dissolving metallic ions from complex e-wastes. These
extraction selectivity (98%). Recently, an efficient ammonia-ammonium microbes have the ability to facilitate metal dissolution through a series
carbonate slurry electrolysis system has also been proposed by Wang of chemical reactions such as acidolysis, redoxolysis, and complexolysis
et al. (2021) for high purity Cu extraction from WPCBs of mobile phones. (Desmarais et al., 2020). Jowkar et al. (2018) reported 100% extraction

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R. Kumari and S.R. Samadder Journal of Environmental Management 320 (2022) 115887

of indium from discarded liquid crystal displays (LCDs) using Acid­ the leaching efficiencies can reach up to 71% for Cu, 96% for Sn, & Pb,
ithiobacillus thiooxidans. Recent studies are more focused on using mixed and 98% for Zn within 240 min under optimized conditions.
culture of microorganisms and combination of microbes with other Direct electro-dissolution of powdered WPCBs was carried out by
chemical lixiviants for maximum extraction of metals from e-wastes. For Guimarães et al. (2014) in an acidic copper sulfate solution to recover
example, Pant et al. (2014) reported first the use of microbes (Serratia Cu. The results indicated that electrolyte stirring and temperature in­
plymuthica) and EDTA for improved metal leaching from waste CRTs. crease favored cathodic recovery of Cu (96%). In another study, Fogarasi
Işıldar et al. (2016) performed a two-step bioleaching process using et al. (2014) investigated a chemical–electrochemical process involving
A. thiooxidans & A. ferrivorans in the first stage and P. fluorescens & acidic ferric chloride solution for simultaneous Cu extraction and Au
P. putida in the second stage for enhanced Cu extraction (98.4%). In separation from WPCBs using two different reactors in series. A leaching
another study, Heydarian et al. (2018) also performed two-step bio­ reactor with a perforated rotating drum was employed for dissolution of
leaching using a mixture of A. thiooxidans and A. ferrrooxidans and base metals and a divided electrochemical reactor was used for regen­
extracted around 99% Li, 89% Ni, and 50% Co under optimized condi­ eration of the leaching solution and for electrowinning of Cu. After
tions. Similar mixed culture bioleaching experiment was also conducted dissolution and recovery of Cu (99.04%), the Au concentration in the
by Priya and Hait (2020) using A. ferrrooxidans and Acidiphilium acid­ residue enhanced 25 times than that in the initial sample. Direct re­
ophilum. The mixed culture demonstrated highest bioleaching effi­ covery of Cu from complex e-wastes through a process combining
ciencies of around 95% for Cu & Zn and 75% for Ni & Pb. . electro-dissolution and electro-deposition was also achieved by Haccu­
Biosorption process is another biological approach for recovering ria et al. (2017).
metals from WPCBs. In various studies, bacteria, fungi, other living or Minimum chemical requirement is one of the advantages of electro-
dead microbial mass, agricultural and plant biomass have been used as recycling process for recovery of metals. Nevertheless, inadequate
biosorbents for recovering metals from the leached solutions of e-wastes. electrical conductivity of WPCBs and high energy consumption during
Varshney et al. (2017) recovered Cd (93.03%), Pb (95.18%), and Ni ball-milling are some of the major limitations that hamper the recovery
(97.08%) from WPCBs using ameliorated wood pulp as biosorbent. In efficiency of this process. Moreover, the recovery process is found un­
another study, Yi et al. (2016) used ethylenediamine-modified suitable for processing complex e-wastes (Guimarães et al., 2014).
persimmon tannin as biosorbent for recovering Au (~100%) and Pd
(~100%) from the leached solution of WPCBs. Sinha et al. (2018) 4.5. Supercritical fluid (SCF) extraction method
demonstrated the biosorption potential of Aspergillus oryzae and Baker’s
Yeast in recovering Cu from WPCBs (>80%); however, the duration In recent years, supercritical fluid (SCF) technology has attracted
required for effective biosorption is quite high. These adsorbed metals much attention for extraction of metals from e-wastes. These SCFs are
were then desorbed from the biosorbents with specific solvents or were the fluids that remain in single-phase even at/above its critical tem­
incinerated. This method is believed as cost-effective and perature and pressure with gas-like diffusion rate & viscosity, and liquid-
environment-friendly, but the efficiency of the process is dependent on like density (Sanyal et al., 2013). The special properties of SCFs such as
selectivity, total metal-binding capacity, stability and renewability of low viscosity, high solubility, high mass transfer coefficient, and high
materials (Awasthi et al., 2019). diffusivity for organics make this method eco-friendly. This technique is
Overall, the process can be considered as a green alternative to suitable for decomposition of organic fractions and recovery of metallic
conventional metallurgical processes because of their lower operational constituents from e-wastes (Xiu et al., 2015).
temperature & energy requirement and better environmental perfor­ Generally, SCF treatment of e-wastes is done either through SCF
mance. However, the challenges of slow kinetics, maintaining the extraction process or through SCF oxidation process. SCF extraction
quality and purity of microbial culture, and low waste load due to mi­ method is mainly used for extraction of metals and smaller molecules of
crobial sensitivity to toxic constituents of e-wastes remained a concern organic materials and SCF oxidation method is used for degrading
in its full scale industrial operation (Işıldar et al., 2018). Few studies organic constituents of e-wastes (Xiu et al., 2013). Several researchers
have investigated the configurations of bioleaching process using bio­ have used supercritical water (SCW) as SCF combined with acid leaching
reactors, but the knowledge for same at large scale is still limited. For for extraction of base metals from WPCBs (Xiu et al., 2013; Golzary and
example, Erust et al. (2021) performed bioleaching of Cu from WPCBs in Abdoli, 2020). SCW has also been used for extraction of precious metals
a semi-pilot reactor system using a consortium of iron and sulfur from e-wastes (Xiu et al., 2015). Liu et al. (2016) used SCF
oxidizing bacteria. Results revealed that consortium efficiently solubi­ oxidation-extraction process for extraction of Ag and Pd from WPCBs.
lized Cu (95%) at a solid/liquid ratio of 10% within 8 days. Another SCW oxidation was used for enrichment of precious metals and super­
project of BiotaWee has also worked on bioleaching at large scale. The critical CO2 was used as an eco-friendly solvent for extraction of
project has implemented 10 to 20 semi-industrial bioreactors for the precious metals resulting in 93.7% and 96.4% extraction of Pd and Ag
recovery of valuable metals from WPCBs in two-step bioleaching process respectively. In another study, Xiu et al. (2017) proposed a method for
using metabolically-engineered cyanogenic bacteria (ARGCON5). The direct recovery of ultrafine Cu from WPCBs using supercritical methanol
leaching efficiency was found to reach 100%, 80% and 60% for Fe, Ni, after extraction of Cu using nitric acid. The reducing capacity of su­
and Cu respectively within 48 h (BiotaWee, 2021). percritical methanol is used to reduce the Cu ions into zero-valent Cu
contained in the leached liquor of waste without any further addition of
4.4. Electrochemical process reductant.
SCF techniques demonstrate promising green reaction and resource
Electrochemical process is another promising technology for recovery option, but these methods still have certain technical short­
extraction of precious, critical and base metals from e-wastes because of comings. In fact, the SCF treatment methods need more operational cost
its minimum environmental impacts and less requirement of chemicals. and energy than that of hydrometallurgical treatment methods. The sole
In this process, dissolution of metals is favored by proton generation at disadvantage of using SCW in acid leaching is the requirement of higher
the anode (Kim et al., 2010). Kim et al. (2011) investigated the leaching temperature (420–440 ◦ C). Further, the corrosion and salt deposition at
behavior of metals such as Cu, Zn, Pb, and Sn from WPCBs using high temperature and pressure are some of the other concerns associated
electro-generated chlorine in HCl solution. The experiment was per­ with this method (Li and Xu, 2019).
formed using two different reactors, viz. a combined reactor equipped
with the facility for simultaneous Cl2 generation and metal leaching, and 4.6. Vacuum metallurgy method
a separate metal leaching reactor connected with the anode compart­
ment of a Cl2 gas generator. The separate leaching reactor revealed that In recent years, the vacuum metallurgical (VM) technique has gained

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R. Kumari and S.R. Samadder Journal of Environmental Management 320 (2022) 115887

popularity for extracting metals from e-wastes. The VM separation years, different ILs have been used as green solvents for metal extraction
technique includes the methods of vacuum evaporation, vacuum from e-wastes. A feasibility study was conducted by Zhu et al. (2012) to
reduction, vacuum sublimation, and vacuum pyrolysis (Ma and Xu, dissolve brominated epoxy resins of WPCBs using the IL 1-ethyl-3-me­
2013). Separation of metals using VM method is based on the difference thylimizadolium tetrafluoroborate [EMIM+][BF−4 ] for recovering cop­
in vapor pressure of the metallic elements present in e-wastes. This per foils and glass fibers. Huang et al. (2014) used
technique is suitable for recovery of elements such as Bi, Sb, Pb, and 1-butyl-3-methyl-imidazolium hydrogen sulfate ([bmim]HSO4) as IL for
other heavy metals from WPCBs (Zhan and Xu, 2012). Niu et al. (2017) leaching of Cu from WPCBs with almost 100% extraction efficiency. In
used vacuum pyrolysis in combination with mechanical− physical sep­ another study, a comparative analysis on extraction efficiencies of five
aration to recover Ta and other materials from waste tantalum capaci­ typical ILs viz. [BSO4HPy]HSO4 (N-sulfobutylpyridinium hydrosulfate),
tors. In another study, Xiang et al. (2015) used vacuum separation and [BSO3HMIm]HSO4 (1-sulfobutyl-3-methylimidazolium hydrosulfate),
inert gas condensation for Zn recovery and preparation of Zn [BSO3HMIm]OTf (N-sulfobutylpyridiniumtrifluoromethanesulfonate),
nano-particles from spent zinc-manganese batteries. [MIm]HSO4 (Methylimidazolium hydrosulfate), [BSO3HPy]OTf (1-sul­
Application of VM technique is not restricted to the recovery of in­ fobutyl-3-methylimidazolium trifluoromethanesulfate) was carried out
dividual elements, but the method can also recover metallic alloys from by Chen et al. (2015a). The results revealed that each of these ILs was
crushed e-wastes (Ruan and Xu, 2016). This method is considered as an capable of extracting almost 100% Cu; however, the extraction of Pb was
environment-friendly method; however, there are certain limitations below 30%. Similar studies were conducted by Zhang et al. (2018a) and
that need to be focused on for enhancing separation and recovery effi­ He et al. (2020) in which, the leaching behavior of Cu from WPCBs was
ciency. For example, the metal oxide layer present on the surface of investigated using different types of acidic ILs. Most of these studies are
particles can influence the separation efficiency and the smaller size of focused only on the extraction of Cu using these ILs from WPCBs and
particles can pose much higher resistance to separation rate than the have neglected other elements. Also, the co-leaching behavior, inter­
larger-sized particles. Moreover, presence of a large amount of other ference of other metals, efficient recovery from leached solution, and
metallic elements can hamper the evaporation rate (Ruan and Xu, regeneration of these ILs should be studied in more details to understand
2016). the practical applicability of ILs.

4.7. Other novel techniques 4.7.3. Integrated metal recovery method


Recently, combinations of two or more metal recovery techniques
Limitations associated with conventional metal recovery techniques (hybrid techniques) have been employed for efficient extraction of
from e-wastes lead to explore and develop more novel green technolo­ metals from e-wastes. Several integrated metal extraction/recovery
gies such as chelation technology, use of ionic liquids, and application of techniques have been developed such as ultrasonically assisted acid
integrated metal extraction approach. A brief description of these novel leaching method (Zhang et al., 2017c), mechano-chemical technology
techniques is given in the following sub-sections. (Niu et al., 2017), combination of hydrometallurgy & biometallurgy
(Pant et al., 2014; Bui et al., 2021), SCF & chemical leaching (Xiu et al.,
4.7.1. Chelation technology 2013) and pyrometallurgy & hydrometallurgy techniques (Havlik et al.,
Chelating agents have been successfully used in the metal extraction 2010). Sinha et al. (2018) employed a combination of bioleaching and
from various contaminated sites. This technique has been adapted biosorption methods as extraction and purification steps followed by
mainly to optimize resource consumption and to minimize negative electro-treatment process to recover Cu from WPCBs. Jadhao et al.
impacts of pollutants on environment. Chelation technique is considered (2020) proposed an integrated approach using pyrolysis and ultra­
as one of the novel greener approaches in e-waste recycling in which, sonication techniques for recovery of metals from e-wastes. The pyrol­
leaching of metallic contents of e-wastes is facilitated by a multi-dentate ysis at a temperature of 400 ◦ C for 20 min resulted in 35% combustible
chelator (lixiviant). The chelator reacts with metals or metallic ions to gases and 60% solid products. The solid products were then treated by
form stable solution of metal-ligand complexes (Chauhan et al., 2015). ultrasonication process to recover the metallic fraction (>90%). In
Limited studies on the use of chelating agents are available for another study, Chen et al. (2020) investigated integrated method of
extraction of metals from e-wastes (Chauhan et al., 2013, 2015). Jadhao low-temperature alkaline smelting and liquid-liquid phase separation to
et al. (2016) used eco-friendly chelation technology to extract Cu from recover metals from WPCBs of mobile phones. The results revealed an
WPCBs and compared the results with conventional acid leaching enhanced separation rate of 99.5%, 97.8%, 95.7%, 88.4%, and 81.6%,
methods. The results revealed that nearly 84% of Cu extraction can be for Al, Si, Zn, Sn, and Pb respectively. Further, the extraction rates of the
achieved using chelation technique while only 27% of Cu can be metals Ag, Au, Cr, and Ni reached 99.8%, 98.1%, 95.6%, and 75.4%
extracted using the traditional acid leaching methods. In another study, respectively.
Sharma et al. (2017) used a similar concept for extraction of Cu and Co Various challenges associated with the individual metal recovery
from WPCBs and mobile batteries under statistically optimized param­ techniques such as high environmental pollution, low efficiency,
eters. Recently, Verma and Hait (2019) employed the chelation method extensive use of chemical reagents, complex workflow, and selective
for extraction of base metals (Cu, Zn, Ni) from WPCBs of obsolete element recovery still remained unsolved. Therefore, more attention is
computers using diethylene triamine pentaacetic acid (DTPA). to be paid towards developing integrated metal recovery techniques for
Further research is required to explore the applicability of chelating efficient and environment-friendly recycling and management of e-
agents for better extraction of metals from e-wastes. Search for new wastes.
biodegradable chelating agents, their degradation pathways and feasi­
bility studies for separation and recovery of chelated metals is also 5. Residual disposal methods
required for development of a more sustainable method of metals re­
covery from e-wastes. The residues obtained both during pre-processing and end-
processing of e-wastes recycling and recovery require special attention
4.7.2. Ionic liquid extraction method due to the toxicity associated with these wastes. In addition, wastewater
Ionic liquids (ILs) have emerged as new class of lixiviants for from e-waste recycling industries needs to be treated before its disposal.
extracting metals from e-wastes. Practical applications of this method These final wastes are usually sent to landfills for its disposal or to
are possible due to their unique properties of negligible vapor pressure, incineration plants for energy production. However, high expenditure,
high thermal stability (<400 ◦ C), chemical stability, and ability to limited landfill space, and environmental and health hazards are some of
dissolve organic and inorganic compounds (Aslanov, 2011). In recent the major concerns of these disposal methods. Focus has been laid on

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R. Kumari and S.R. Samadder Journal of Environmental Management 320 (2022) 115887

conversion of e-wastes residual plastics into organic products using extraction of Cu using the ILs and have neglected other elements.
hydrothermal treatment (Zhao et al., 2018). This treatment technique For actual field application, the various aspects of metal recovery
has been utilized by various researchers in enhancing the recycling techniques need to be addressed. Firstly, the techniques should be
potential of e-wastes (Yoon et al., 2020). Another technique, plasma feasible for commercialization especially for small & medium-sized en­
treatment has also been introduced as a more environment friendly terprises of developing countries. The feasibility can be ensured by
method of residual waste treatment. Cubas et al. (2014) reported focusing on the process optimization, techno-economic analysis, and
disposal of plasma treated e-wastes residuals into a secured landfill as a scale-up studies of these metal recovery techniques. It is evident from
safer procedure. Use of plasma technology has its own benefits such as Table 3 that most of the industrial and scale-up techniques available for
robust installation, rapid heating, more stable energy, reduced emis­ recycling of e-wastes in developed nations are based on pyrometallur­
sions, more economical and environment-friendly disposal (Sanito et al., gical, hydrometallurgical, or combination of these two processes. While
2021). In recent years, some pilot-scale investigations of plasma treat­ in developing countries like India, the recycling process is mostly
ment of e-waste residual have been done (Szałatkiewicz, 2016). A restricted to pre-processing stage only. Despite the technological ad­
detailed review on the residual treatment and disposal of e-waste using vancements, the higher operational & capital cost, lower efficiency, and
plasma technology has been done by Sanito et al. (2021). metal loss due to variable feed compositions remained a concern for the
scale-up of these techniques. Very limited studies are available on in­
6. Critical discussion on the various metal recovery techniques dustrial scale application and on economic evaluation of SCF extraction
method. Also, limited scale-up studies based on electrochemical and
Realization of the importance of metal recovery from e-wastes as an biometallurgical methods are available despite their high recovery ef­
effective and sustainable management step has resulted improvements ficiency and better environmental performance than the existing in­
in different metal recovery techniques in the recent decades. For dustrial recycling practices (Table S5). Thus, further studies are required
example, advancements from manual to mechanical dismantling with an to explore possibility of industrial application of these methods partic­
automated sensor-based sorting (Chen et al., 2013; Marconi et al., ularly in developing countries. Secondly, a thorough research is required
2019), cryogenic grinding (Zhou et al., 2016), selective to establish a scientific, closed-loop, and complete metal recovery sys­
crushing-screening (Phengsaart et al., 2020), etc. are evident. Also, ad­ tem. This can be achieved by understanding the recyclability of various
vances in different metallurgical techniques in the form of shift towards components of e-wastes followed by prioritization of the metals to be
the utilization of less corrosive reagents, other organic, and bio lixiviants recovered using appropriate treatment and recovery methods. For
with similar or higher recovery efficiencies can also be observed from example, a well-designed pretreatment method such as a combination of
the literature (as summarized in Tables S2 and S3). However, these mechano-physical technology can be adapted for efficient separation of
technologies still have certain challenges that need to be addressed for metallic and NMFs to avoid emissions of toxic gases and minimization of
further improvements. Major concerns of these technologies are the residues resulting from NMFs of e-wastes. Recycling technologies can
environmental, economic, and social sustainability which require also be integrated based on the physical and chemical properties of e-
further studies. A comparative assessment of different metal recovery wastes. Though attempts have been made to develop economical and
techniques based on these parameters is presented in Table S5. Metal environment-friendly metal recycling techniques, still there is huge
recovery from e-wastes is itself a very complex process and the hetero­ scope to improve the sustainability of the recovery processes. Applica­
geneous nature of these wastes makes it even more complex. Thus it is tion of single technology may not be adequate for recovering metals
essential to consider all these parameters for accurate evaluation and efficiently from complex e-wastes. However, integrated metal recovery
prediction of the sustainability of these techniques. Sustainability can be methods can be proved as potential metal recovery methods from e-
assessed using LCA studies of these different techniques. Various LCA wastes. Systematic integration of two or more methods for recovering
tools such as SimaPro and GaBi have been used so far to evaluate the metallic fractions from e-wastes can even be more feasible in terms of
environmental impacts of different metal recovery techniques of both economic and environmental aspects.
e-wastes. These tools use different life cycle impact assessment (LCIA)
methods such as Tool for the Reduction and Assessment of Chemical and 7. Conclusion
Other Environmental Impacts (TRACI), International Reference Life
Cycle Data (ILCD), CML, Environmental Development of Industrial The present study critically reviewed the different pre-treatment and
Products (EDIP), and ReCiPe to model the environmental impacts of the metal recovery methods from e-wastes. Following conclusive remarks
various processes (S. No. 3 of Table S5). The most commonly used have been made as per the analysis in this review:
models are USEtox, USES-LCA, EUTREND, EASEWASTE, and RAINS10.
Literature survey revealed that most of the studies are focused on re­ i. Selective and automatic disassembly of components has been
covery of single element; but the extraction efficiency and purity of the recommended for e-wastes containing high metal contents to
recovered metals and the loss of valuable resources remained a concern. enhance recovery efficiency. Further, temperature-controlled
It is evident from Table S2 that most of the chemical leaching systems crushing with a milling size below 150 mm is generally sug­
were focused on recovering either Cu or precious metals and when gested for effective separation of non-metals from metals.
attempted to recover other metals parallelly, the recovery efficiency was ii. For physical separation of metallic and NMFs, density-based
found insignificant. However, leaching using organic acids was found separation methods are usually preferred. However, the latest
efficient to extract rare earth metals, base metals, and other heavy developments including corona electrostatic separators are also
metals from e-wastes (S. No. 14, 16 of Table S2). Thus, potential of more gaining popularity for separation of metallic and NMFs of e-
such types of organic acids need to be evaluated for further improve­ wastes.
ment of extraction efficiency. As the biometallurgical approach is green iii. Significant improvements have been made in traditional methods
and eco-friendly recovery method, thus, this method needs to be such as pyrometallurgical and hydrometallurgical techniques of
explored more to overcome the lower recovery rates. The process effi­ e-waste recycling; still, more improvement is required for feasible
ciency can be improved by optimization of the parameters as achieved application of these techniques at industrial scale with minimum
by Jowkar et al. (2018) for indium recovery (S. No. 9 of Table S3). In environmental impacts.
addition, use of mixed microbial culture can further enhance the re­ iv. Extensive research for biometallurgical, SCF, chelation, and IL
covery efficiency (S. No. 6, 10 of Table S3). Further studies are also leaching methods is also required because of their compatibility
required on ILs and chelating agents based extraction of elements from as effective substitutes for these conventional recovery tech­
e-wastes as most of the previous studies have focused only on the niques. Also, focus should be laid on scaling up the

11
R. Kumari and S.R. Samadder Journal of Environmental Management 320 (2022) 115887

Table 3
Details of the industrial scale technologies available for recycling of e-wastes.
S. Industry (Location) Type of e-waste Recycling technique Materials Remark Reference
No. recycled recovered

1. Forrec- WEEE Large household Manual dismantling and mechanical Fe, plastics, non- The recycling unit has arrangements Forrec
Recycling Plant appliances, TVs, pre-treatment ferrous metals for the air flow and dust control system (2021)
(Italy) CRTs, etc. during grinding as well as noise control
and soundproofing system.
2. Aurubis Recycling Electrical and Pretreatment followed by Cu, Ni, Sn, Pb, and The batch time is short due to quick Aurubis
Center (Germany, electronic scrap. pyrometallurgy and electrolysis other precious melting process in the bath melting (2021)
North America, Asia) method metals furnace.
3. Umicore (North Cell phones, laptops, Smelting, leaching, electrowinning, Base metals (Cu, The recycling unit has treatment Umicore
America, Europe, and other small IT precious metals refining (PMO), base Ni, Pb), precious facility for the byproducts generated (2021)
Asia Pacific, Latin devices without metals operations (BMO): blast metals, secondary from PMO as well as emission (dust,
America, Middle East, batteries. furnace and lead refinery and the metals (Sn, Bi, Sb) gasses, and dioxins) control system.
and Africa) special metal plants
4. Boliden (Sweden, Dismantled and pre- Rönnskär and Kaldo furnace Au, Ag, Cu, Pd, Ni, Melted plastics from e-wastes during Boliden
Finland, Norway, treated e-wastes. (Pyrometallurgy and Se, Zn, and Pb smelting are used as a source of energy. (2021)
Ireland) Hydrometallurgy). The heat generated is partially reused
as district heating in the plant area and
the remaining heat is supplied to the
local district heating system. The
recycling unit is equipped with
advanced systems to clean process
gases and discharge water.
5. UWin Nanotech PCBs. Automatic desoldering, mechanical Cu, Au, Ag, Pd, and The recycling unit uses cyanide-free UWin
(Japan, USA, China, pre-treatment and hydrometallurgy Sn chemical methods and is integrated Nanotech
Taiwan) with automated processes, thereby (2019)
making the recovery of precious metals
more effective.
6. UNIVAQ’s pilot plant PCBs, CPUs, Hydrometallurgy, cementation/ Cu, Ag, Au, and tin The process is suitable for e-wastes rich Fenix (2020)
[FENIX] (Italy) electrical connectors, precipitation, and electrowinning oxide in precious metals (i.e. larger than
mother boards and methods 500–800 g/t of Au) and is not very
other kinds of e- efficient for grinded materials.
wastes.
7. E-Parisarra Private PCBs, toner Manual dismantling and other Plastics, glass, and The method of recycling is restricted to E-Parisarra
Limited (India) cartridges, tube mechanical pre-treatment methods metals manual dismantling, other mechanical (2021)
lights, CRTs, etc. sorting, and density-based separation
methods.

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